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About ten years ago, chemically fueled systems have emerged as a new class of synthetic materials with tunable properties. Yet, applications of these materials are still scarce. In part, this is due to an incomplete characterization of the viscoelastic properties of those materials, which has – so far – mostly been limited to assessing their linear response under shear load. Here, we fill some of these gaps by comparing the viscoelastic behavior of two different, carbodiimide fueled Fmoc-peptide systems. We find that both, the linear and non-linear response of the hydrogels formed by those Fmoc-peptides depends on the amount of fuel driving the self-assembly process – but hardly on the direction of force application. In addition, we identify the concentration of accumulated waste products as a novel, so far neglected parameter that crucially affects the behavior of such chemically fueled hydrogels. With the mechanistic insights gained here, it should be possible to engineer a new generation of dynamic hydrogels with finely tunable material properties that can be tailored precisely for such applications, where they are challenged by mechanical forces.

Viscoelastic behavior of chemically fueled supramolecular hydrogels under load and influence of reaction side products